2021 Fiscal Year Annual Research Report
Developing isolated single metal ion coordinated by carbon nitrides for photocatalytic H2O2 production based on Time-Dependent Density Function Theory
| Project/Area Number |
20J13064
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| Research Institution | Shinshu University |
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Principal Investigator |
滕 鎮遠 信州大学, 先鋭領域融合研究群先鋭材料研究所, 特別研究員(PD)
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| Project Period (FY) |
2020-04-24 – 2022-03-31
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| Keywords | Photocatalysis / H2O2 production / Molecular engineering / Single-atom catalyst / Population analysis / Time-dependent DFT |
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| Outline of Annual Research Achievements |
We demonstrate a polarization engineering strategy by grafting (thio)urea functional groups onto covalent triazine frameworks (CTFs), giving rise to significantly promoted charge separation/transport and obviously enhanced proton transfer. Our calculation studies reveal the performance is attributed to the prominently enhanced 2-electron oxygen reduction reaction by improved charge separation and highly concentrated holes at the thiourea site.
We also a prepared a flat and uniform polycrystalline Cu3BiS3 (CBS) thin film on a molybdenum-coated glass (Mo-SLG) by spray pyrolysis deposition for generation of hydrogen peroxide (H2O2). The photoelectrochemically (PEC) synthesis proceeds by an indirect 2e－ ORR initial formation of superoxide, which is disproportionate to H2O2.
We calculated the water oxidation ability and its influence on photocatalytic oxidation of CH4 over symmetrically coordinated cobalt single-atom. It is revealed that the single-cobalt-atom PCN photocatalyst with 2N and 2C coordinated Co center possesses a desired electronic configuration for one electron transfer water oxidation reaction during photocatalysis.
The activation of water for boosting the mass transfer of H to form H2O2 is found to be the rate-determined step during the 2e- ORR process on triazine sites. Taking SAC_Au-KPCN as an example, the overlap of K 4s and Au 5d orbitals generated a shallow-trapped energy level for accumulation of highly-concentrated holes at Au sites, thus leading to an significantly accelerated H2O activation and a remarkably boosted activity for H2O2 production.
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| Research Progress Status |
令和3年度が最終年度であるため、記入しない。
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| Strategy for Future Research Activity |
令和3年度が最終年度であるため、記入しない。
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